Title: Selective Detection of Intermediate-Amplitude Motion by Solid-State NMR

Journal Article · · Journal of Physical Chemistry. B
ORCiD logo [1]; ORCiD logo [2]
  1. Massachusetts Institute of Technology, Cambridge, MA (United States); Massachusetts Institute of Technology
  2. Massachusetts Institute of Technology, Cambridge, MA (United States)
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The coexistence of rigid and mobile molecules or molecular segments abounds in biomolecular assemblies. Examples include the carbohydrate-rich cell walls of plants and intrinsically disordered proteins that contain rigid β-sheet cores. In solid-state nuclear magnetic resonance (NMR) spectroscopy, dipolar polarization transfer experiments are well suited for detecting rigid components, whereas scalar-coupling experiments are well suited for detecting highly mobile components. However, few NMR methods are available to detect the segments that undergo intermediate-amplitude fast motion. Here, we introduce two NMR experiments, a two-dimensional T2H-filtered CP-hCH correlation and a three-dimensional J-INADEQUATE CCH correlation, to observe this intermediate-amplitude motion. Both experiments involve 1H detection under fast magic-angle spinning (MAS). By combining 1H transverse relaxation (T2H) filters with dipolar polarization transfer, we suppress the signals of both highly rigid and highly mobile species, thus revealing the signals of intermediate mobile species. 1H detection under fast MAS is crucial for distinguishing the different motional amplitudes. Here, we demonstrate these techniques on several plant cell wall samples and show that they allow the selective detection and resolution of certain hemicellulose and pectin signals, which are usually masked by the signals of the rigid cellulose and the highly dynamic pectins in purely dipolar and scalar NMR spectra.

Research Organization:
Massachusetts Institute of Technology, Cambridge, MA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0001090
OSTI ID:
2459318
Journal Information:
Journal of Physical Chemistry. B, Journal Name: Journal of Physical Chemistry. B Journal Issue: 10 Vol. 128; ISSN 1520-6106
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (49)

The Dynamic Structure of Filamentous Tau journal October 2011
Fast Magic‐Angle‐Spinning NMR Reveals the Evasive Hepatitis B Virus Capsid C‐Terminal Domain** journal June 2022
Characterization of different water pools in solid-state NMR protein samples journal September 2009
Protein resonance assignment at MAS frequencies approaching 100 kHz: a quantitative comparison of J-coupling and dipolar-coupling-based transfer methods journal August 2015
Spinning faster: protein NMR at MAS frequencies up to 126 kHz journal January 2019
Fast MAS 1H–13C correlation NMR for structural investigations of plant cell walls journal September 2019
1H-N.m.r. study of enzymically generated wheat-endosperm arabinoxylan oligosaccharides: structures of hepta- to tetradeca-saccharides containing two or three branched xylose residues journal January 1992
High-performance solvent suppression for proton detected solid-state NMR journal May 2008
Probing membrane protein structure using water polarization transfer solid-state NMR journal October 2014
High-resolution proton-detected NMR of proteins at very fast MAS journal April 2015
Multidimensional solid-state NMR spectroscopy of plant cell walls journal September 2016
Hidden motions and motion-induced invisibility: Dynamics-based spectral editing in solid-state NMR journal September 2018
Hydration and Dynamics of Full-Length Tau Amyloid Fibrils Investigated by Solid-State Nuclear Magnetic Resonance journal May 2020
Solid-State NMR Investigations of Extracellular Matrixes and Cell Walls of Algae, Bacteria, Fungi, and Plants journal December 2021
1H-Detected Biomolecular NMR under Fast Magic-Angle Spinning journal May 2022
Structure and Interactions of Plant Cell-Wall Polysaccharides by Two- and Three-Dimensional Magic-Angle-Spinning Solid-State NMR journal February 2011
Structure and Dynamics of Brachypodium Primary Cell Wall Polysaccharides from Two-Dimensional 13 C Solid-State Nuclear Magnetic Resonance Spectroscopy journal April 2014
Use of 13C MAS NMR to Study Domain Structure and Dynamics of Polysaccharides in the Native Starch Granules journal June 2003
2D and 3D 15 N− 13 C− 13 C NMR Chemical Shift Correlation Spectroscopy of Solids:  Assignment of MAS Spectra of Peptides journal November 2000
NMR Measurement of Signs and Magnitudes of C-H Dipolar Couplings in Lecithin journal March 1995
Observation of Highly Flexible Residues in Amyloid Fibrils of the HET-s Prion journal September 2006
Water–Polysaccharide Interactions in the Primary Cell Wall of Arabidopsis thaliana from Polarization Transfer Solid-State NMR journal July 2014
Structural Rearrangements of Membrane Proteins Probed by Water-Edited Solid-State NMR Spectroscopy journal January 2009
A Novel Tool for Probing Membrane Protein Structure:  Solid-State NMR with Proton Spin Diffusion and X-Nucleus Detection journal May 1998
Resonance Assignments for Solid Peptides by Dipolar-Mediated 13 C/ 15 N Correlation Solid-State NMR journal July 1998
A Method for Measuring Heteronuclear ( 1 H− 13 C) Distances in High Speed MAS NMR journal March 2000
Inclusion of the C-Terminal Domain in the β-Sheet Core of Heparin-Fibrillized Three-Repeat Tau Protein Revealed by Solid-State Nuclear Magnetic Resonance Spectroscopy journal May 2021
pH- and Calcium-Dependent Aromatic Network in the SARS-CoV-2 Envelope Protein journal April 2022
Water Distribution, Dynamics, and Interactions with Alzheimer’s β-Amyloid Fibrils Investigated by Solid-State NMR journal April 2017
Investigation of Molecular Motions by Lee-Goldburg Cross-Polarization NMR Spectroscopy journal June 2002
Information on Bond Orientation Distributions in Lipids and Liquid Crystals from Segmental Order Parameters journal January 1996
Molecular architecture of fungal cell walls revealed by solid-state NMR journal July 2018
Fluent molecular mixing of Tau isoforms in Alzheimer’s disease neurofibrillary tangles journal May 2022
Architecture of the dynamic fungal cell wall journal October 2022
The peptide hormone glucagon forms amyloid fibrils with two coexisting β-strand conformations journal June 2019
Structure and drug binding of the SARS-CoV-2 envelope protein transmembrane domain in lipid bilayers journal November 2020
Water orientation and dynamics in the closed and open influenza B virus M2 proton channels journal March 2021
Solid-state NMR spectroscopy journal January 2021
The fuzzy coat of pathological human Tau fibrils is a two-layered polyelectrolyte brush journal December 2012
In vitro 0N4R tau fibrils contain a monomorphic β-sheet core enclosed by dynamically heterogeneous fuzzy coat segments journal July 2019
Structural characterization of the core of the paired helical filament of Alzheimer disease. journal July 1988
Solid-state NMR investigations of cellulose structure and interactions with matrix polysaccharides in plant primary cell walls journal September 2015
Solid-State 13C Nuclear Magnetic Resonance Characterization of Cellulose in the Cell Walls of Arabidopsis thaliana Leaves journal June 1996
Wall Structure and Wall Loosening. A Look Backwards and Forwards: Fig. 1. journal January 2001
Cellulose-Pectin Spatial Contacts Are Inherent to Never-Dried Arabidopsis Primary Cell Walls: Evidence from Solid-State Nuclear Magnetic Resonance journal June 2015
Gradients in Wall Mechanics and Polysaccharides along Growing Inflorescence Stems journal October 2017
Microtubule-binding core of the tau protein journal July 2022
Amyloid fibril structures of tau: Conformational plasticity of the second microtubule-binding repeat journal July 2023
Looking Beyond the Core: The Role of Flanking Regions in the Aggregation of Amyloidogenic Peptides and Proteins journal December 2020

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